SENSORS AND ACTUATORS B-CHEMICAL
·
2016
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IF 4.758
Weiwei Meng,Lei Dai,Wei Meng,Huizhu Zhou,Yuehua Li,Zhangxing He,Ling Wang
Mixed-potential type NH 3 sensors were fabricated using La 10 Si 5.5 Al 0.5 O 27 (LSAO) consisting of a porous layer and a dense layer as solid electrolyte and TiO 2 as the sensing electrode. The effect of a LSAO porous layer and TiO 2 phase transformation on sensor performances was investigated. The porous layer of LSAO electrolyte obviously enhanced sensor performance. Compared with the sensor without a LSAO porous layer, the sensor with LSAO porous layer exhibited larger responding potential values and higher sensitivity due to the enhanced three phase interface length. Anatase-TiO 2 (a-TiO 2 ) based sensor exhibited better sensing performance than rutile-TiO 2 (r-TiO 2 ) based sensor at the examined temperature range. A-TiO 2 transformation toward r-TiO 2 resulted in poor sensing performances of the sensor. The best sensing characteristics were achieved for the NH 3 sensor with a-TiO 2 sensing electrode calcined at 900 °C for 3 h. The potential values of the sensor response to NH 3 linearly depended on the logarithm of NH 3 concentrations at 450–600 °C and the sensitivity reached 169.7 mV/decade in the range of 50–400 ppm at 500 °C. At the same time, the sensor exhibited well anti-interference capability to H 2 , NO, CH 4 and CO 2 , but a little cross-sensitivity toward NO 2 was observed. High temperature treatment (>900 °C) caused a-TiO 2 transformation into r-TiO 2 and V 2 O 5 additions were conducive to TiO 2 phase transformation.
研究领域:
材料科学
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传感器技术
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环境监测
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu-Wei Zhao,Wei Zeng,Sheng-Qi Su,Si-Dong Zhang,Si-Jie Guo,Jian-Hua Qiu,Yong-Gang Sun,An-Min Cao,Xi-Jie Lin
Surface coating as an effective strategy has been extensively utilized to enhance the surface/interface stability of cathode for lithium-ion batteries. As widely recognized, the electrochemical performance of coated cathode is greatly dependent on the properties of coating layer. Rational design on the structure and composition of coating layer becomes crucial. Here, a unique “island-bridge” shaped Zr-based coating layer has been constructed through a facile synthetic protocol. This coating layer composes of several high-crystalline ZrO 2 nanoparticles and a thin low-crystalline zirconium hydroxide layer that connects these nanoparticles, forming a typical “island-bridge” structure. The successful formation of such a unique coating layer was demonstrated to be related to the usage amount of Zr source and the calcined temperature. The novel “island-bridge” coating has been successfully applied to modify the surface of LiCoO 2 , showing excellent capability on improving the electrochemical performance. The unique “island-bridge” structure coating induces the formation of a triple-phase interface, namely island-cathode-bridge interface. Theoretical calculation suggests that such an island-cathode-bridge triple-phase interface can effectively reduce the Li + diffusion energy, leading to favorable Li + transportation kinetics and suppressed cathode-electrolyte interface evolution. Furthermore, this “island-bridge” layer can well prevent direct contact between LiCoO 2 and electrolyte, enhancing the surface/interface stability, resulting in improved cyclic performance. This work provides new insights into the rational design of surface coating for high-energy density cathodes.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-11
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IF 12.121
Zhang Qizhan,Zhou Minghua,Ren Gengbo,Li Yawei,Li Yanchun,Du Xuedong
Hydrogen peroxide (H 2 O 2 ) synthesis by electrochemical oxygen reduction reaction has attracted great attention as a green substitute for anthraquinone process. However, low oxygen utilization efficiency (<1%) and high energy consumption remain obstacles. Herein we propose a superhydrophobic natural air diffusion electrode (NADE) to greatly improve the oxygen diffusion coefficient at the cathode about 5.7 times as compared to the normal gas diffusion electrode (GDE) system. NADE allows the oxygen to be naturally diffused to the reaction interface, eliminating the need to pump oxygen/air to overcome the resistance of the gas diffusion layer, resulting in fast H 2 O 2 production (101.67 mg h -1 cm -2 ) with a high oxygen utilization efficiency (44.5%–64.9%). Long-term operation stability of NADE and its high current efficiency under high current density indicate great potential to replace normal GDE for H 2 O 2 electrosynthesis and environmental remediation on an industrial scale.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Huining Huang,Qitao Zhang,Run Shi,Chenliang Su,Yulin Wang,Jiaqi Zhao,Tierui Zhang
Solar-to-chemical energy conversion is a challenging subject for renewable energy storage. Solar-driven hydrogen peroxide (H 2 O 2 ) synthesis is a sustainable and potentially economic technology. Despite great efforts in catalyst engineering, photocatalytic H 2 O 2 production is usually limited by the sluggish oxygen diffusion and H 2 O 2 decomposition side reactions, leading to poor apparent photocatalytic H 2 O 2 production efficiency. Herein, we developed a fluid triphase system that enables both the efficient interfacial oxygen mass transfer and the inhibited H 2 O 2 decomposition side reactions. Such a synergistic effect endowed a residue-free H 2 O 2 production rate of 6.03 μmol h −1 from pure water and oxygen without using any sacrificial agent or additive, with over 120 h continuous irradiation stability. We further designed a photosynthesis-concentration tandem system to produce high concentration H 2 O 2 (10 mM), which demonstrated an effective water disinfection capability as a representative application.
研究领域:
能源化学
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环境科学
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光合作用研究
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zimou Liu,Kuiling Li,Lie Liu,Hang Song,Yong Zhang,Mike Tebyetekerwa,Xiwang Zhang,Ke Wang,Lili Xu,Jun Wang
Electrosynthesis of hydrogen peroxide (H 2 O 2 ) presents a sustainable alternative to the anthraquinone process, while the transition to applying this process at industrial-relevant currents remains a significant challenge. Most studies tried to solve it by catalysts modulations, whereas we found that the accessibility to the gaseous O 2 , might be the crux of this matter. Herein, we developed a series of membrane-based gas diffusion electrodes (Mem-GDEs) with varied O 2 accessibility. Their endurable currents were found to be well correlated with the O 2 mass transferability. By constructing high O 2 -accessible triphasic interfaces, Mem-GDE achieved a recorded current density , 1.4 A cm −2 , with the current efficiency higher than 80.6 %. It was also verified for the first time that the insufficient O 2 triggered a severe flooding problem and thus further deteriorate the O 2 mass transfer. This study highlights the importance of O 2 accessibility and provides new insights into triphasic interfaces construction for realizing industrial-used H 2 O 2 -generated electrodes.
研究领域:
化学工程
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电化学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yujun Ju,Hua Li,Ze Wang,Hanwen Liu,Shuhui Huo,Shan Jiang,Sicong Duan,Yonggang Yao,Xiaoquan Lu,Fengjuan Chen
Organic pollutants in wastewater have raised great concerns because of their considerable risk to human health and the ecosystem. Although Fenton reaction of advanced oxidation process represents a promising water treatment strategy. However, continuous consumption and low utilization efficiency of H 2 O 2 limit its practical application. Herein, we propose photocatalytic in-situ production and activation H 2 O 2 at triphase interface to reach excellent removal efficiency for contaminants. The triphase interface configuration allows oxygen rapid diffusion from the air to the surface of photocatalyst and avoids the problem of poor mass transfer of oxygen in solution. Meanwhile, using the Z-type heterojunction MIL-101(Fe)/g−C 3 N 4 as model photocatalysts could largely promote the photo-induced electrons and holes separation efficiency to further improve reaction efficiency. As a result, the triphase photocatalytic system achieved an in-situ H 2 O 2 production rate of 4370 μmol h −1 (greater than5 times higher than the diphase control) and a superior degradation efficiency for organic pollutants (model pollutant: methyl orange, concentration: 10 ppm, 99% removal rate in 130 min, while only 21% in diphase control) with a 17.5 times higher reaction rate constant. Therefore, the triphase photocatalytic system realized the highly efficient degradation of organic pollutants in wastewater by solar-driven, in-situ generation and activation of H 2 O 2 with high catalytic activity and minimized oxygen transport limitation, thus providing a green and sustainable strategy for wastewater treatment and broadly environmental remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Pu Wang,Jiaqi Zhao,Run Shi,Xuerui Zhang,Xiangdong Guo,Qing Dai,Tierui Zhang
As a promising environmental treatment technology, photocatalysis has been investigated for decades and even tentatively practiced in actual large-scale applications. However, most researches focus on photocatalytic kinetics (excitation, charge transfer, and surface reaction) but ignore the significant impact of oxygen interfacial mass transfer for photocatalytic aerobic oxidation in aqueous media. Here, we use finite element simulation to demonstrate that during photocatalysis, the remained local oxygen concentration for photocatalysts at a gas-liquid-solid triphase interface is much higher than that dispersed in a bulk liquid phase. Photocatalyst consisting of Au/TiO 2 nanoparticles supported at triphase interface shows a non-diffusion limited charge separation for oxygen photoactivation, therefore achieving a photodegradation efficiency of about 85% toward bisphenol A. Furthermore, we develop a flowing triphase photocatalytic system that exhibits a tunable one-way photodegradation efficiency from 10% to 60% and a photostability for up to 50 h of continuous irradiation, further demonstrating the potential for large-scale applications.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Industrial Chemistry & Materials
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2024
·
IF 0
Huige Chen,Zhenhua Li,Chao Zhou,Run Shi,Tierui Zhang
The exothermic characteristic of the water-gas-shift (WGS) reaction, coupled with the thermodynamic constraints at elevated temperatures, has spurred a research inclination towards conducting the WGS reaction at reduced temperatures. Nonetheless, the challenge of achieving efficient mass transfer between gaseous CO and liquid H2O at the photocatalytic interface under mild reaction conditions hinders the advancement of the photocatalytic WGS reaction. In this study, we introduce a gas–liquid–solid triphase photocatalytic WGS reaction system. This system facilitates swift transportation of gaseous CO to the photocatalyst's surface while ensuring a consistent water supply. Among various metal-loaded TiO2 photocatalysts, Rh/TiO2 nanoparticles positioned at the triphase interface demonstrated an impressive H2 production rate of 27.60 mmol g−1 h−1. This rate is roughly 2 and 10 times greater than that observed in the liquid–solid and gas–solid diphase systems. Additionally, finite element simulations indicate that the concentrations of CO and H2O at the gas–liquid–solid interface remain stable. This suggests that the triphase interface establishes a conducive microenvironment with sufficient CO and H2O supply to the surface of photocatalysts. These insights offer a foundational approach to enhance the interfacial mass transfer of gaseous CO and liquid H2O, thereby optimizing the photocatalytic WGS reaction's efficiency.
研究领域:
化学工程
·
材料科学
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环境科学
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jianxin Liu,Rui Li,Xiang Zu,Xiaochao Zhang,Yunfang Wang,Yawen Wang,Caimei Fan
Photocatalysis can produce NH 3 using N 2 and H 2 O at room temperature and atmospheric pressure, which has been considering as a safe, clean, and sustainable NH 3 synthesis. However, the poor solubility and slow diffusion rate of N 2 in water severely limited the nitrogen activation efficiency. Herein, we solve this problem by developing a hydrophilic-hydrophobic structure photocatalyst with gas-liquid-solid triphase reaction interface, where hydrophilic Bi 4 O 5 Br 2 is deposited on the surface of hydrophobic ZIF-8 to form a novel Bi 4 O 5 Br 2 /ZIF-8 composite photocatalyst. Such triphase interface architecture allows the direct delivery of N 2 from gas phase to the photocatalytic reaction interface replaced the diffusion of N 2 through the liquid phase. This rapid supply of N 2 can efficiently capture photoinduced electrons, thereby promoting the utilization efficiency of photo-induced electrons and the nitrogen fixation activation. This novel Bi 4 O 5 Br 2 /ZIF-8(30%) composite photocatalyst with good triphase contact performance shows obviously improved photocatalytic nitrogen fixation activity 327.338 μmol·L −1 ·h −1 ·g −1 (3.6 times than that of Bi 4 O 5 Br 2 ). Furthermore, efficient molecular nitrogen activation by Bi 4 O 5 Br 2 /ZIF-8 further brings out an attractive potential to improve other gas-consumption reactions, such as CO 2 reduction, according to this concept of triphase direct contact.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Peng Huang,Nan Li,Liang Zeng,Yujie Zhu
The long-term goal of electrochemical ammonia (NH3) synthesis under ambient conditions is to replace the Haber–Bosch process. One of the biggest challenges in this field is that the N≡N triple bond is too stable to be activated. Therefore, most research is mainly focused on the development of advanced electrocatalysts to address this challenge. However, the extremely low solubility and slow diffusion of N2 molecules in aqueous electrolytes are usually overlooked. Here, the Bi-loaded Cu hollow microtube with a porous structure is reported as the gas diffusion electrode for N2 electroreduction. Compared with the conventional planar electrode configurations, the hollow gas diffusion electrode (HGDE) possesses unique advantages in breaking through the mass transfer limit of low-solubility gases. It can also provide abundant electrochemically active sites due to its porous structure, forming a gas–liquid–solid three-phase interface that is conducive to electrocatalytic reactions. Besides, the adjustable N2/H3O+ at the three-phase interface can further help enhance the reaction activity and selectivity. As a result, the Bi-loaded Cu HGDE exhibits an NH3 yield of 4.6 μg h–1 cm–2 and a Faradaic efficiency of 5.8% at −0.4 V (vs RHE, reversible hydrogen electrode). This study may stimulate interest in optimizing the electrode structure and developing types of electrodes for efficient electrochemical ammonia synthesis.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhiru Suo,Yuan Zhuang,Yanjun Zhao,Peng Zhou,Fushun Li,Binbin Huang,Chen Qu,Wenhui Li,Chuandong Wu,Jiemin Liu
Advanced oxidation processes (AOPs, such as Fenton) coupled with wet scrubbers are powerful and eco–friendly for VOCs treatment. However, challenges remain in the efficient removal of hydrophobic VOCs due to the extremely high gas-liquid mass transfer resistance. Herein, we constructed a “gas-solid-liquid triple-phase interface” in a Fenton wet scrubber via fabricating a new amphiphilic catalyst (PAN@Fe 3 O 4 @Nafion), which allows to capture gas bubbles and directly convey the VOCs to catalytic active center through gas transport and bypass the gas-liquid mass transfer (rate–determining) step. Compared with system with the unmodulated catalyst, the removal efficiency of hydrophobic styrene in the triple-phase interface Fenton wet scrubber was improved by 69.0%, the intermediates were dominated by small–molecule fatty acids (98.0%), and the outlet CO 2 concentration and H 2 O 2 consumption increased by 22.1% and 19.6%, respectively. Notably, mechanism analysis via confocal laser scanning microscopy and contact angle measurements revealed the arrangement of hydrophilic and hydrophobic regions on the catalyst surface. Moreover, the affinity ability of bubbles was 2.5 times greater and the mass transfer enhancement factor reached 2.2 in the triple-phase interface Fenton wet scrubber system. This study provides a new avenue for overcoming the gas-liquid mass transfer resistance of hydrophobic VOCs in AOP wet scrubbers.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Huimin Yang,Cheng Nan,Nan Gao,Wenjing Zhou,Fanfan Gao,Dai Dong,Danyang Dou,Yujie Liu,Zhenhai Liang,Donghua Yang
Photoelectrochemical nitrogen reduction (PEC NRR) provides a clean and sustainable method for the production of NH 3 under environmental conditions. However, low reaction efficiency remains a major challenge due to the presence of competitive hydrogen evolution reactions (HER). Herein, nanocomposites (SNP/MSO) with three-phase interface were prepared by loading hydrophilic SnO 2 nanoparticles (SNP) on hydrophobic MoS 2 (MSO) obtained by surface modification with silicomolybdic acid. The hydrophobic interface eliminated the transport barrier of N 2 in the liquid phase to the reaction center, inhibiting HER since the lowered contact area with the liquid proton. Meanwhile, the heterojunction structure formed between MSO and SNP accelerated the effective electron transfer . The synergistic effect of the triphase interface structure and electron transfer structure contributed to the high NH 3 yield (19.6 μg h −1 mg −1 ) and FE (40.34%) of SNP/10MSO in the photoelectrochemical system. Compared with the nanocomposites (SNP/MSI) prepared by hydrophilic MoS 2 , FE was significantly increased by 10 percentage points.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）